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Title: Theory of femtosecond coherent double-pump single-molecule spectroscopy: Application to light harvesting complexes

We develop a first principles theoretical description of femtosecond double-pump single-molecule signals of molecular aggregates. We incorporate all singly excited electronic states and vibrational modes with significant exciton-phonon coupling into a system Hamiltonian and treat the ensuing system dynamics within the Davydov D{sub 1} Ansatz. The remaining intra- and inter-molecular vibrational modes are treated as a heat bath and their effect is accounted for through lineshape functions. We apply our theory to simulate single-molecule signals of the light harvesting complex II. The calculated signals exhibit pronounced oscillations of mixed electron-vibrational (vibronic) origin. Their periods decrease with decreasing exciton-phonon coupling.
Authors:
;  [1] ; ;  [2]
  1. Division of Materials Science, Nanyang Technological University, 50 Nanyang Avenue, Singapore 639798 (Singapore)
  2. Department of Chemistry, Technische Universit√§t M√ľnchen, Garching D-85747 (Germany)
Publication Date:
OSTI Identifier:
22415698
Resource Type:
Journal Article
Resource Relation:
Journal Name: Journal of Chemical Physics; Journal Volume: 142; Journal Issue: 16; Other Information: (c) 2015 AIP Publishing LLC; Country of input: International Atomic Energy Agency (IAEA)
Country of Publication:
United States
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL AND ANALYTICAL CHEMISTRY; COMPLEXES; COUPLING; ELECTRONS; EXCITONS; HAMILTONIANS; MOLECULES; OSCILLATIONS; PHONONS; SPECTROSCOPY; VISIBLE RADIATION